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WO2008013094A1 - Article moulé et son procédé de fabrication - Google Patents

Article moulé et son procédé de fabrication Download PDF

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Publication number
WO2008013094A1
WO2008013094A1 PCT/JP2007/064240 JP2007064240W WO2008013094A1 WO 2008013094 A1 WO2008013094 A1 WO 2008013094A1 JP 2007064240 W JP2007064240 W JP 2007064240W WO 2008013094 A1 WO2008013094 A1 WO 2008013094A1
Authority
WO
WIPO (PCT)
Prior art keywords
molded article
thermoplastic resin
fiber
composite material
reinforced composite
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2007/064240
Other languages
English (en)
Japanese (ja)
Inventor
Atsuki Tsuchiya
Masato Honma
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Toray Industries Inc
Original Assignee
Toray Industries Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Toray Industries Inc filed Critical Toray Industries Inc
Priority to EP07790994.3A priority Critical patent/EP2047983B1/fr
Priority to US12/309,736 priority patent/US20090208721A1/en
Priority to CN2007800284336A priority patent/CN101495307B/zh
Publication of WO2008013094A1 publication Critical patent/WO2008013094A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

Links

Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/04—Layered products comprising a layer of synthetic resin as impregnant, bonding, or embedding substance
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/04—Reinforcing macromolecular compounds with loose or coherent fibrous material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C45/00—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor
    • B29C45/14—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor incorporating preformed parts or layers, e.g. injection moulding around inserts or for coating articles
    • B29C45/14778—Injection moulding, i.e. forcing the required volume of moulding material through a nozzle into a closed mould; Apparatus therefor incorporating preformed parts or layers, e.g. injection moulding around inserts or for coating articles the article consisting of a material with particular properties, e.g. porous, brittle
    • B29C45/14786—Fibrous material or fibre containing material, e.g. fibre mats or fibre reinforced material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C65/00—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor
    • B29C65/02—Joining or sealing of preformed parts, e.g. welding of plastics materials; Apparatus therefor by heating, with or without pressure
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/01—General aspects dealing with the joint area or with the area to be joined
    • B29C66/05—Particular design of joint configurations
    • B29C66/10—Particular design of joint configurations particular design of the joint cross-sections
    • B29C66/11—Joint cross-sections comprising a single joint-segment, i.e. one of the parts to be joined comprising a single joint-segment in the joint cross-section
    • B29C66/112—Single lapped joints
    • B29C66/1122—Single lap to lap joints, i.e. overlap joints
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/40—General aspects of joining substantially flat articles, e.g. plates, sheets or web-like materials; Making flat seams in tubular or hollow articles; Joining single elements to substantially flat surfaces
    • B29C66/41—Joining substantially flat articles ; Making flat seams in tubular or hollow articles
    • B29C66/43—Joining a relatively small portion of the surface of said articles
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
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    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
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    • B29C66/731—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the intensive physical properties of the material of the parts to be joined
    • B29C66/7311—Thermal properties
    • B29C66/73115—Melting point
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
    • B29C66/70—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material
    • B29C66/73—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset
    • B29C66/731—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the intensive physical properties of the material of the parts to be joined
    • B29C66/7311—Thermal properties
    • B29C66/73117—Tg, i.e. glass transition temperature
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    • B29C66/00—General aspects of processes or apparatus for joining preformed parts
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    • B29C66/739—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the material of the parts to be joined being a thermoplastic or a thermoset
    • B29C66/7392—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the material of at least one of the parts being a thermoplastic
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    • B29C66/739—General aspects of processes or apparatus for joining preformed parts characterised by the composition, physical properties or the structure of the material of the parts to be joined; Joining with non-plastics material characterised by the intensive physical properties of the material of the parts to be joined, by the optical properties of the material of the parts to be joined, by the extensive physical properties of the parts to be joined, by the state of the material of the parts to be joined or by the material of the parts to be joined being a thermoplastic or a thermoset characterised by the material of the parts to be joined being a thermoplastic or a thermoset
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2535/00—Medical equipment, e.g. bandage, prostheses or catheter
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2605/00—Vehicles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2605/00—Vehicles
    • B32B2605/08—Cars
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2605/00—Vehicles
    • B32B2605/18—Aircraft
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2367/00—Characterised by the use of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Derivatives of such polymers
    • C08J2367/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/249921—Web or sheet containing structurally defined element or component
    • Y10T428/249924—Noninterengaged fiber-containing paper-free web or sheet which is not of specified porosity
    • Y10T428/249933—Fiber embedded in or on the surface of a natural or synthetic rubber matrix

Definitions

  • the present invention relates to a molded article formed by joining a fiber reinforced composite material and a thermoplastic resin member, and has an impact adhesive strength between the fiber reinforced composite material and the thermoplastic resin member.
  • the present invention relates to an improved molded article and a manufacturing method thereof.
  • a fiber-reinforced composite material using a thermosetting resin as a matrix resin is a material excellent in mechanical properties and light weight.
  • This fiber-reinforced composite material is widely used as a constituent member of various molded products including constituent members of aircraft and automobiles.
  • thermoplastic resin members formed by resin injection molding, parts with relatively simple shapes are formed by fiber reinforced composite materials, and these parts are joined together by joining Goods are being used.
  • Patent Document 1 and Patent Document 2 disclose a resin frame assembly excellent in impact resistance.
  • This assembly is a molded product in which a functional component and a thermoplastic resin member are integrated.
  • a maleimide-based or polycarbonate-based polymer Z vinyl-based polymer z rubber-like polymer Z a frame member made of a resin composition that also has reinforcing fiber strength, while a metal or the like is applied to the same resin composition.
  • Functional parts that have been insert-molded are manufactured, and then these parts are joined together by thermal welding between the greases used in each of the parts.
  • Patent Document 2 disclose a resin frame assembly excellent in impact resistance.
  • This assembly is a molded product in which a functional component and a thermoplastic resin member are integrated.
  • a maleimide-based or polycarbonate-based polymer Z vinyl-based polymer z rubber-like polymer Z a frame member made of a resin composition that also has reinforcing fiber strength, while a metal or the like is applied to the same resin composition.
  • Patent Document 3 discloses a fiber reinforced composite material laminate that can be easily and firmly welded to another member, and a thermoplastic resin member that forms the laminate and a frame member, etc. An adhesion technique for increasing the bonding strength of the film and an integrally molded product formed thereby are described. However, the technique described in Patent Document 3 is mainly intended to increase the adhesion, particularly to improve the adhesion to the polyamide resin material. It ’s not enough.
  • Patent Document 1 Japanese Patent Laid-Open No. 11 138641
  • Patent Document 2 Japanese Patent Laid-Open No. 11-268130
  • Patent Document 3 WO 2004 / 060658A 1 Publication
  • An object of the present invention is to provide a molded article in which a fiber-reinforced composite material and a thermoplastic resin member are joined and integrated, and a method for producing the same, which are particularly excellent in impact resistance.
  • the molded product of the present invention for achieving the above object is as follows.
  • a molded article comprising an integrated thermoplastic resin member ( ⁇ ), wherein the thermoplastic resin (A) and the fiber-reinforced composite material (I) have a joint surface formed by the molded product.
  • thermoplastic resin (A) has a concavo-convex shape and the maximum impregnation thickness h of the thermoplastic resin (A) into the fiber-reinforced composite material (I) is the above, and the thermoplastic resin (A) has a tensile breaking strength of 25 MPa or more and a tensile breaking elongation of 200% or more, and impact bonding at the joint between the fiber-reinforced composite material (I) and the thermoplastic resin member ( ⁇ ). Strength is 3000jZm Molded product that is 2 or more.
  • the tensile elongation at break of the thermoplastic resin (A) is preferably 350% or more.
  • the impact strength force of the thermoplastic member ( ⁇ ) is preferably 200 jZm or more, more preferably 300 J / m or more.
  • the impact strength force of the fiber reinforced composite material (I) is preferably 500 J Zm or more. It is preferable that the minimum thickness t of the thermoplastic resin (A) is 10 / z m to 500 ⁇ m.
  • the thermoplastic resin (A) 1S is composed of one or more kinds of polyester resin, and at least one of the polyester resins has a polyethylene terephthalate component in a hard segment, And a copolyester containing one or both of polybutylene terephthalate components and a polytetramethylene glycol component as a diol component constituting the soft segment.
  • At least one kind of the polyester resin is one or two kinds selected from the primary amino group, the epoxy group, and the acid anhydride group. It preferably has a functional group structure.
  • the glass transition temperature of the polyester resin Tg force It is preferable that the formula satisfies 0 ° C ⁇ Tg ⁇ 80 ° C.
  • Melting point of polyester resin Tm force Tm force 120 ° C ⁇ Tm ⁇ 180 ° C and melt viscosity 7-1 at temperature (Tm + 10) ° C is 500Pa 's ⁇ ⁇ 1 It is preferable that ⁇ 2, OOOPa's is satisfied. More preferably, the polyester resin satisfies the melting point Tm force formula 120 ° C ⁇ Tm ⁇ 160 ° C. Further, the melt viscosity r? 2 at a temperature of 250 ° C of the polyester resin is more preferably 300 Pa's or less.
  • thermoplastic resin member ( ⁇ ) is one or more resin compositions selected from polycarbonate resin, ABS resin, and thermoplastic elastomer resin. .
  • thermoplastic resin member ( ⁇ ⁇ ) is made of a portion (III) having radio wave permeability.
  • the electric field shielding power Od B to 15 dB of the portion (III) having radio wave permeability is preferable.
  • the part having radio wave permeability (III) force It is preferably formed of a member reinforced with non-conductive fibers.
  • the part having radio wave permeability ( ⁇ ) force Shaped by a member reinforced with glass fiber with a content of 30% to 70% by weight It is preferable that it is made.
  • a substantial thickness of the fiber-reinforced composite material (I) is 0.1 mm to 0.6 mm. It is preferable that the continuous reinforcing fibers in the fiber-reinforced composite material (I) are carbon fibers.
  • thermosetting matrix resin in the fiber-reinforced composite material (I) is an epoxy resin.
  • the molded article of the present invention is preferably used as a molded article in electrical and electronic equipment, office automation equipment, home appliances, medical equipment, automobile parts, aircraft parts, or building materials. Further, the molded product of the present invention is preferably used as a molded product in a personal computer casing or a mobile phone casing.
  • the frame portion when a frame portion is present, the frame portion is formed by the thermoplastic resin member (II), and is formed on at least a part of the thermoplastic resin member (II). In addition, it is preferable that a portion ( ⁇ ) having radio wave permeability is disposed.
  • thermoplastic member (II) having a radio wave transmitting portion (III) is as follows.
  • thermoplastic resin in the portion (wax) having radio wave permeability and the thermoplastic resin in the thermoplastic resin member (wax) are the same type of resin.
  • the fiber-reinforced composite material (I) containing continuous reinforcing fibers and thermosetting matrix resin is firmly bonded and integrated.
  • FIG. 1 is a schematic cross-sectional view in the thickness direction of one embodiment of a molded article of the present invention.
  • FIG. 2 is a schematic perspective view of a test piece when measuring the impact adhesive strength of the molded article of the present invention.
  • FIG. 3 is a schematic exploded perspective view of a test piece when measuring the impact adhesive strength and adhesive strength of the molded article of the present invention.
  • FIG. 4 is a perspective view of an example of a personal computer case using the molded article of the present invention and a partial cross-sectional view in the thickness direction.
  • FIG. 5 is a schematic perspective view of a test piece when measuring the impact adhesive strength of the molded article of the present invention.
  • FIG. 6 is a perspective view of a part of an example of a mobile phone casing using the molded article of the present invention.
  • FIG. 7 is a cross-sectional view taken along the line SI-S1 of FIG.
  • thermoplastic resin member (II) 2b Reinforcing fiber located farthest from thermoplastic resin member (II)
  • FIG. 1 One embodiment of the molded article of the present invention is shown in FIG.
  • the molded product 1 is heated on at least a part of the surface of the fiber-reinforced composite material (I) including the continuous reinforcing fiber 2 and the thermosetting matrix resin 3 and the fiber-reinforced composite material (I). It consists of a thermoplastic resin member (II) joined and integrated by the plastic resin (A).
  • thermoplastic resin (A) is impregnated in the gaps between the continuous reinforcing fibers 2 of the fiber-reinforced composite material (I) and joined with the thermosetting matrix resin 3 of the fiber-reinforced composite material (I).
  • the molded product 1 has a structure in which a part of the reinforcing fiber 2 of the fiber reinforced composite material (I) is included in the layer of the thermoplastic resin (A). And speak.
  • the joint surface 4 between the thermoplastic resin (A) and the thermosetting matrix resin 3 of the fiber reinforced composite material (I) has an uneven shape in the cross section in the thickness direction of the molded product 1.
  • the joint surface 4 has an uneven shape because part of the reinforcing fibers 2 of the reinforcing fibers 2 is embedded in the thermoplastic resin (A) in a part of the longitudinal direction. It means that the other part following it is embedded by the thermosetting matrix resin 3. This state is not observed in the cross section shown in FIG. 1, but can be clearly understood by observing a cross section perpendicular to the cross section.
  • the reinforcing fiber 2 has an anchoring effect for preventing delamination between the thermoplastic resin (A) and the fiber-reinforced composite material (I).
  • the thermoplastic resin (A) is joined to the fiber reinforced composite material (I) by the thermoplastic resin (A) and integrated into the thermoplastic member (II) and the fiber reinforced composite material (I). It also has the effect of inhibiting the peeling between the two!
  • the maximum impregnation thickness h of the thermoplastic resin (A) into the fiber-reinforced composite material (I) is 10 ⁇ m or more. It has been.
  • the maximum impregnation thickness h is more preferably 20 / zm or more, and further preferably 30 / zm or more.
  • the upper limit value of the maximum impregnation thickness h is not particularly limited, but if it is about 1,000 m, there is no practical problem.
  • the thermoplastic resin (A) has a tensile strength at break of 25 MPa or more. This requirement in the molded article 1 means that the thermoplastic resin (A) is strong as the adhesive itself.
  • the tensile strength at break of the thermoplastic resin (A) is more preferably 30 MPa or more, and further preferably 35 MPa or more.
  • the upper limit of the tensile strength at break of the thermoplastic resin (A) is not particularly limited, but considering that it is a thermoplastic resin (A), there is no practical problem if it is about lOOMPa.
  • the tensile elongation at break of the thermoplastic resin (A) is 200% or more. This requirement in the molded article 1 means that the thermoplastic resin (A) functions effectively as an adhesive by absorbing the load.
  • the tensile elongation at break of the thermoplastic resin (A) is more preferably 300% or more, still more preferably 350% or more.
  • the upper limit of the tensile elongation at break of the thermoplastic resin (A) is not particularly limited, but considering that it is a thermoplastic resin (A), there is no practical problem if it is about 1,000%.
  • the impact bonding strength of the joint 5 between the fiber-reinforced composite material (I) and the thermoplastic resin member ( ⁇ ) is set to 3, OOOjZm 2 or more. This requirement for molded product 1 means that when impact is applied to molded product 1, delamination at joint 5 is suppressed.
  • the impact adhesive strength of the joint 5 between the fiber-reinforced composite material (I) and the thermoplastic resin member ( ⁇ ) is more preferably 4, OOOjZm 2 or more, and further preferably 5, OOOjZm 2 or more.
  • the upper limit of the impact bond strength of the joint 5 between the fiber reinforced composite material (I) and the thermoplastic resin member ( ⁇ ) is not particularly limited, but from the viewpoint of exhibiting excellent impact bond strength, 30 , OOOjZm 2 or so, there is no practical problem.
  • the impact strength of the thermoplastic resin member ( ⁇ ) is 200 jZm or more. Are preferred. This requirement in the molded product 1 means that even when an impact is applied to the molded product 1, the thermoplastic resin member ( ⁇ ) does not break and has excellent impact resistance. .
  • the impact strength of the thermoplastic resin member ( ⁇ ⁇ ) is more preferably 300 jZm or more, and further preferably 500 jZm or more.
  • the upper limit of the impact strength of the thermoplastic resin member ( ⁇ ) is not particularly limited, but considering that it is a thermoplastic resin member ( ⁇ ), there is a practical problem if it is about 1, OOOJ / m. Absent.
  • thermoplastic resin ( ⁇ ) and the thermoplastic resin (A) need not be clear! / ⁇ .
  • thermoplastic rosin having the same composition may be used for each.
  • the impact strength of the fiber-reinforced composite material (I) is 300 jZm or more. This requirement in the molded article 1 means that even when an impact is applied to the molded article 1, the fiber-reinforced composite material (I) does not break and has excellent impact resistance.
  • the impact strength of the fiber reinforced composite material (I) is more preferably 500 jZm, and still more preferably 700 jZm or more.
  • the upper limit of the impact strength of the fiber reinforced composite material (I) is not particularly limited, but if it is about 3, OOOjZm, there is no practical problem.
  • the minimum thickness t of the thermoplastic resin (A) is preferably 10 m to 500 m. This requirement in the molded article 1 means that an adhesive layer for adhesion to other members by the thermoplastic resin (A) is preferably secured.
  • the thickness t of the thermoplastic resin (A) is more preferably 20 ⁇ m to 300 ⁇ m, still more preferably 40 ⁇ m to 100 ⁇ m.
  • the adhesive strength between the fiber-reinforced composite material (I) and the thermoplastic resin member (II) is preferably 12 MPa or more at 25 ° C. This requirement for part 1 means that the impact resistance of the whole part is increased.
  • the adhesive strength between the fiber reinforced composite material (I) and the thermoplastic resin member ( ⁇ ) is more preferably 15 MPa or more, and further preferably 2 OMPa or more.
  • the upper limit of the adhesive strength is not particularly limited, but if it is about 40 MPa, there is no practical problem.
  • Thermoplastic resin in molded product 1 (A) force It consists of one or two or more polyester resins, and at least one polyester resin among the polyester resins is polyethylene terephthalate in the hard segment. Ingredients and polybutylene terephthalate ingredients One of these is preferably a copolyester containing both components and a polytetramethylene glycol component as the diol component constituting the soft segment.
  • This copolymer polyester comprises, as a hard segment, 5 to 80% by weight of a polyester component comprising an aromatic or alicyclic cyclic dicarboxylic acid and a diol represented by the following structural formula 1. And a polyester component comprising, as a soft segment, an aromatic ring type or alkylene dicarboxylic acid having 2 to 10 carbon atoms and a diol in which R is a linear alkylene oxide among diols represented by the following structural formula 1: Preferably, it is a copolyester containing 20% to 95% by weight.
  • R represents a linear or branched structure represented by C H (n is an integer of 2 to 10) n 2n
  • the polyester resin is a mixture of two or more kinds of polyester resins, it is preferable that at least one polyester resin is a copolymer polyester having the above structure.
  • the aromatic ring-type dicarboxylic acid constituting the hard segment includes terephthalic acid, isophthalic acid, orthophthalic acid, 1,5 naphthalenedicarboxylic acid, 2,6 naphthalenedicarboxylic acid, noraphthalene-dicarboxylic acid, Examples include sodium sulfoisophthalate.
  • the alicyclic dicarboxylic acids constituting the hard segment include 1,4-cyclohexanedicarboxylic acid, 1,3 cyclohexanedicarboxylic acid, 1,2 cyclohexanedicarboxylic acid, 4-methyl-1,2 cyclohexane. Hexanedicarboxylic acid.
  • Examples of the diol represented by Structural Formula 1 include ethylene glycol, diethylene glycol, triethylene glycol, polyethylene glycol, polytetramethylene glycol, propylene glycol, 1,3 propanediol, and 2-methyl-1,3 propane.
  • alkylenedicarboxylic acid having 2 to 10 carbon atoms constituting the soft segment examples include fumaroleic acid, maleic acid, itaconic acid, succinic acid, gnoretanolic acid, adipic acid, suberic acid, azelaic acid, sebacic acid, Examples include dodecanedioic acid and dimer acid.
  • the structure of the hard segment preferably includes one or both of a polyethylene terephthalate component and a polybutylene terephthalate component, which are resin components that are widely used industrially.
  • the content is preferably in the range of 20% to 70% by weight, preferably in the range of 10% to 80% by weight, in the case of including either one or both. Further preferred.
  • Polytetramethylene glycol is preferably included as the diol component in order to impart flexibility to the coconut resin.
  • this polyester resin is one or more selected from the primary terminal amino group, epoxy group and acid anhydride group of one end or both ends of polyester resin. It preferably has two types of functional group structures. These reactive functional groups preferably act to improve adhesion to various materials not only by the formation of a covalent bond by a chemical reaction, but also by electrostatic force due to hydrogen bonds and high polarity.
  • the polyester resin is a mixture of two or more polyester resins, it is preferable that at least one polyester resin has the above terminal structure.
  • the polyester resin may be used alone, or may be a thermoplastic resin composition containing other additive components.
  • Additives include inorganic fillers, flame retardants, conductive additives, crystal nucleating agents, UV absorbers, antioxidants, vibration control agents, antibacterial agents, insect repellents, deodorants, anti-coloring agents, heat stabilizers , Mold release agents, antistatic agents, plasticizers, lubricants, colorants, pigments, dyes, foaming agents, antifoaming agents and coupling agents.
  • the polyester resin satisfies the glass transition temperature Tg force formula 0 ° C ⁇ Tg ⁇ 80 ° C.
  • the glass transition temperature Tg is within this range, the mobility of molecules near room temperature is suppressed, and it becomes possible to develop high adhesive strength as a strong polyester resin.
  • the glass transition temperature Tg satisfies the formula 10 ° C ⁇ Tg ⁇ 80 ° C, more preferably the formula 25 ° C ⁇ Tg ⁇ 80 ° C.
  • the polyester resin is a mixture of two or more kinds
  • the lowest glass transition temperature Tg is treated as the glass transition temperature Tg of the polyester resin.
  • Polyester resin has a melting point Tm that satisfies the formula 120 ° C ⁇ Tm ⁇ 180 ° C. A force that satisfies the formula 120 ° C ⁇ Tm ⁇ 160 ° C. Power More preferred.
  • Tm melting point
  • the polyester resin is a mixture of two or more kinds, and there are two or more melting points Tm, it is necessary to bond the polyester resin after sufficiently melting it from the viewpoint of The highest melting point Tm is treated as the melting point Tm of the polyester resin.
  • Polyester resin is generated by a parallel plate with a diameter of 20 mm at a temperature (Tm + 10) ° C. Its melt viscosity at 0.005 J is 7? 1 force 500Pa 's ⁇ ⁇ 1 ⁇ 2, OOOPa- s Is preferably satisfied. If the melt viscosity 7-1 at a temperature (Tm + 10) ° C is within the above range, the adhesive spreads well on the adherend and prevents the adhesive from flowing out, ensuring both processability and securing adhesive strength. It becomes possible.
  • the melt viscosity 7-1 is preferably 600 Pa's to 1,800 Pa's, more preferably 700 Pa's to 1,600 Pa's.
  • melt viscosity 7-1 In order to make the melt viscosity 7-1 within the above range, a method of adjusting the molecular weight of the polyester resin, or a copolymer polyester using two or more kinds of dicarboxylic acids and two or more kinds of diols, It is possible to control the melt viscosity r? 1 by controlling the regularity of the molecular chain and increasing or decreasing the crystallinity. For example, by lowering the molecular weight, the melt viscosity r? 1 can be reduced, and components that can exhibit flexibility such as a dicarboxylic acid component having a large number of carbon atoms and a diol component having a large number of carbon atoms can be used. When a polyester resin is prepared as a material, it is possible to reduce the melt viscosity 7-1.
  • melt viscosity of 7 to 1 when the polyester resin is a mixture of two or more, two types of melt viscosities r? 1 cannot be obtained.
  • the viscosity of the mixture that does not need to be distinguished is measured as it is to obtain a melt viscosity of 7-1.
  • the polyester resin preferably has a melt viscosity r? 2 of 300 Pa's or less at a generated torque of 0.005 J by a parallel plate having a diameter of 20 mm at a temperature of 250 ° C.
  • a melt viscosity of 7 to 2 in this range makes it easy to press-cage polyester resin into a sheet, which is very effective in the construction process when using polyester resin as an adhesive. is there.
  • the lower limit of the melt viscosity r? 2 is not particularly limited, but the melt viscosity r? 2 is usually lPa's or more considering that the polyester resin is a high molecular weight product.
  • the melt viscosity 7-2 is preferably 250 Pa's or less, more preferably 200 Pa's or less.
  • thermoplastic resin member (II) constituting the molded article 1 is composed of one or more resin compositions selected from polycarbonate resin, ABS resin, and thermoplastic elastomer resin. I like it! /
  • thermoplastic elastomer examples include styrene-based elastomer, olefin-based elastomer, polyvinyl chloride-based elastomer, urethane-based elastomer, polyester-based elastomer, and polyamide-based elastomer.
  • the constituent resin of the thermoplastic resin member (II) is an alloy resin of polycarbonate resin or polycarbonate resin and ABS resin.
  • thermoplastic resin member (II) may be composed of the thermoplastic resin alone.
  • the thermoplastic resin member (II) improves the strength of the thermoplastic resin member ( ⁇ ) and improves the mechanical properties of the molded article 1.
  • the thermoplastic resin member (II) may contain reinforcing fibers.
  • the reinforcing fiber include glass fiber, carbon fiber, metal fiber, aromatic polyamide fiber, polyaramid fiber, alumina fiber, silicon carbide fiber, boron fiber, and basalt fiber. These reinforcing fibers are used alone or in combination of two or more. When reinforcing fibers are included, the fiber content is preferably 5% to 60% by weight.
  • thermoplastic resin (A) is preferably a polyester resin having a high affinity with these resin compositions.
  • the polyester resin constituting the thermoplastic resin (A) preferably has a number average molecular weight of 10,000 to 30,000 in order to ensure the strength and fluidity of the resin itself. .
  • the number average molecular weight is more preferably 12,000 to 28,000, still more preferably 15,000 to 25,000.
  • the form of the continuous reinforcing fiber 2 in the fiber-reinforced composite material (I) constituting the molded article 1 is not particularly limited, and a reinforcing fiber bundle composed of a large number of reinforcing fibers, and the fiber bundle strength. Combining them, such as a structured cloth, a reinforcing fiber bundle in which a large number of reinforcing fibers are arranged in one direction (unidirectional fiber bundle), and a unidirectional cloth in which this unidirectional fiber bundle force is also constructed. And those in which a plurality of layers are arranged. Among these, from the viewpoint of substrate productivity, cloth and unidirectional fiber bundles are preferably used.
  • the reinforcing fiber bundle may be composed of a plurality of fiber fibers having the same form, or may be composed of a plurality of fibers having different forms.
  • the number of reinforcing fibers constituting one reinforcing fiber bundle is usually 300 to 48,000, but considering the production of the base material, it is preferably 300 to 24,000, and more preferably 1, 000 to 12,000.
  • the continuous reinforcing fiber 2 is a reinforcing fiber continuous over a length of 10 mm or more in at least one direction.
  • the reinforcing fibers 2 do not have to be continuous over the entire length of the fiber reinforced composite material (I) or the entire width of the fiber reinforced composite material (I). , You may be divided on the way.
  • the fiber material of the reinforcing fiber 2 used includes glass fiber, carbon fiber, metal fiber, aromatic polyamide fiber, polyaramid fiber, alumina fiber, silicon carbide fiber, boron fiber, basalt fiber, and the like. . These may be used alone or in combination of two or more. These fiber materials may be subjected to surface treatment. Surface treatment includes metal deposition treatment, treatment with a coupling agent, treatment with a sizing agent, and additive adhesion treatment. Among these fiber materials, conductive fiber materials are also included. As the fiber material, carbon fiber having a low specific gravity and high strength and high elastic modulus is preferably used.
  • the substantial thickness of the fiber-reinforced composite material (I) is 0.1 mm to 0.6 mm.
  • thermosetting matrix resin 3 in the fiber reinforced composite material (I) unsaturated polyester, butyl ester, epoxy, phenol (resole type), urea melamine
  • polyimides, bismaleimides, cyanate esters, etc. there are copolymers, modified products, and resins blended with at least two of these.
  • an elastomer or a rubber component may be added.
  • the epoxy resin is also preferable from the viewpoint of the mechanical properties of the molded product.
  • the epoxy resin is included as a main component of the thermosetting matrix resin 3 in order to express its excellent mechanical properties. It is preferable.
  • the fiber-reinforced composite material (I) preferably has an impact resistant layer having a tear strength of 80 NZmm or more on at least a part of the surface or inside thereof. Thereby, the impact resistance of the molded product 1 is further improved. Since the fiber reinforced composite material (I) has an impact resistant layer on at least a part of the surface or inside thereof, the fiber reinforced composite material (I) cracks when impact is applied, and the fiber reinforced composite of the impact object. Damage due to penetration of material (I) is suppressed.
  • the tear strength of the impact resistant layer is more preferably lOONZmm or more, and even more preferably 150NZmm or more.
  • the material for forming the impact-resistant layer is not particularly limited, but from the viewpoint of light weight and moldability, the material is preferably greaves.
  • Examples of greases that form an impact resistant layer include impact resistance Polyester resin is an impact resistant polyamide resin.
  • thermoplastic resin member (wax) also has a part (III) force having radio wave permeability. Further, it is preferable that the electric field shielding power OdB to 15 dB of the portion (III) having radio wave permeability.
  • the radio wave transmitting portion (III) is formed of a member reinforced with a non-conductive fiber. Further, it is preferable that the part (III) having radio wave permeability is formed of a member reinforced with glass fiber having a content of 30 to 70% by weight.
  • Molded product 1 has a frame portion, and the frame portion is the thermoplastic resin member.
  • a portion (III) formed of (II) and having radio wave permeability is disposed on at least a part of the frame portion.
  • the molded article 1 is preferably used in electrical / electronic equipment, office automation equipment, home appliances, medical equipment, automobile parts, aircraft parts, or building materials.
  • the molded product 1 is preferably used in a personal computer casing or a mobile phone casing.
  • the frame portion ( ⁇ ) formed of the thermoplastic resin member ( ⁇ ) of the molded product 1 in order to reduce the weight.
  • the amount be as small as possible.
  • the fiber reinforced composite material (I) can be sufficiently bonded and supported by the frame part ( ⁇ ).
  • the projected area of the joint portion between the fiber reinforced composite material (I) and the frame portion (II) is preferably 5 to 75% of the projected area of the fiber reinforced composite material (I). More preferably, it is 10% to 60% of the projected area, and more preferably 20% to 50% of the projected area.
  • the fiber-reinforced composite material (I) is preferably small in size and lightweight, and its maximum projected area is 10,000 mm 2 or less. It is preferable that there is. More preferably, it is 8,000 mm 2 or less, and still more preferably 6,000 mm 2 or less.
  • thermoplastic resin (A) when the fiber-reinforced composite material (I) and the thermoplastic resin member (II) are integrally formed through the thermoplastic resin (A), the integral part thereof is used.
  • Techniques and methods for molding Thermal welding, vibration welding, ultrasonic welding, laser welding, insert injection molding, outsert injection molding, and the like are preferably used, and outsert molding and insert molding are preferably used from the viewpoint of the molding cycle. .
  • thermoplastic resin (A) h (2)
  • the maximum impregnation thickness h is the reinforcing fiber 2a located closest to the thermoplastic resin member (II) among the reinforcing fibers 2 located in the layer of the thermoplastic resin (A). And the thermoplastic resin member (i) is defined as the distance between the reinforcing fiber 2b located farthest from the cable.
  • the maximum impregnation thickness h is determined by cutting out a cross-section portion containing thermoplastic resin (A) from the molded product to a size of 5 mm x 5 mm, creating a test piece, and taking an image of the obtained cross-section with an optical microscope. The maximum impregnation thickness h was measured from the obtained image and obtained. The image magnification is 300 times. Note that a scanning electron microscope (SEM) or a transmission electron microscope (TEM) can be used instead of the optical microscope. If the thermoplastic rosin (A) is clearly observable, it may be dyed as necessary to enhance the contrast of observation.
  • SEM scanning electron microscope
  • TEM transmission electron
  • the minimum thickness t of the thermoplastic resin (A) is the thermoplastic resin (A) that exists between the thermoplastic resin member ( ⁇ ) and the fiber-reinforced composite material (I). Is defined as the smallest of the thicknesses.
  • the minimum thickness t is obtained by cutting out a cross-sectional part containing the thermoplastic resin (A) from the molded product with a size of 5 mm x 5 mm, creating a test piece, and photographing the obtained cross-section with an optical microscope. The minimum thickness t is measured from the obtained image. The magnification of image shooting is 300 times. Note that a scanning electron microscope (SEM) or a transmission electron microscope (TEM) can be used instead of the optical microscope. If the thermoplastic rosin (A) is clearly observable, it may be dyed as necessary to enhance the contrast of observation.
  • SEM scanning electron microscope
  • TEM transmission electron microscope
  • thermoplastic resin (A) the tensile strength at break of the thermoplastic resin (A) is measured based on the specifications after cutting a test piece of the size specified in IS0527 from the molded product 1. If a test piece of the specified size is not obtained from molded product 1, a film with a width of 5 mm and a length of 20 mm is prepared separately using thermoplastic resin (A), and this film is used as the test piece. Also good! [0089] (4) Tensile elongation at break of thermoplastic resin (A):
  • thermoplastic resin (A) the tensile elongation at break of the thermoplastic resin (A) is measured based on the specifications after cutting a test piece of the size specified in IS0527 from the molded product 1. If a test piece of the specified size is not obtained from molded product 1, a film with a width of 5 mm and a length of 20 mm is prepared separately using thermoplastic resin (A), and this film is used as the test piece. Also good!
  • FIG. 2 shows the dimensions of the test piece 21 to be used.
  • L1 is the length of the thermoplastic resin member (II)
  • W1 is the width of the fiber-reinforced composite material (I) and the thermoplastic resin member ( ⁇ )
  • T1 is the thermoplastic resin member ( ⁇ ) Is the thickness.
  • the test piece 21 is cut out from the part of the molded product 1 where these dimensions can be taken as much as possible.
  • the fiber-reinforced composite material (I) of the cut specimen 21 is thin, it may be difficult to use it for the test as it is.
  • the cut specimen 51 and the aluminum plate 52 are joined using a one-pack type epoxy adhesive (manufactured by Sumitomo 3EM Co., Ltd., EW2070). Let's say 53. At this time, the thickness T3 of the aluminum plate 52 is 20 mm.
  • the test is performed in accordance with the requirements of IS09653 by setting the test piece 21 or 53 so that the hammer hits the thermoplastic resin member ( ⁇ ) side.
  • the impact absorption energy measured by the measurement method based on IS09653 is divided by the adhesion area to obtain the impact adhesion strength.
  • the adhesive strength between the fiber reinforced composite material (I) and the thermoplastic resin member (II) is as follows from the molded product 1 to the fiber reinforced composite material (I) and the thermoplastic resin member ( ⁇ ) as shown in Fig. 3.
  • the part where the joints are joined and integrated is cut out as a test piece 31 and, in principle, measured in accordance with IS04587.
  • L3 in the test piece 31 is the length of the bonded portion, and M is a fiber-reinforced composite material.
  • the size of the test piece 31 is the size based on the provisions of IS04587. However, if a test piece of that size cannot be obtained from the molded product 1, it is a molding that allows each dimension to be as large as possible. Use a test piece cut out from the product 1 part.
  • the obtained specimen 31 is subjected to a lap shear tensile test in accordance with IS04587. By dividing the measured bond breaking load by the bond area 10, the bond strength is calculated.
  • the impact strength (Izod impact strength with notch) of fiber reinforced composite material (I) is measured in accordance with the provisions of AS TMD256. However, the size of the specimen obtained from molded product 1 If there is not enough clearance, cut the test piece from the part of the molded product 1 where the width, thickness, and length can be taken as much as possible, and perform measurement.
  • a plate-like part having a width of 10 mm, a length of 64 mm, and a thickness of 1 mm is cut out from the fiber-reinforced composite material (I) portion of the molded product 1 and subjected to the notch shape processing described in ASTM D256.
  • a test piece was obtained.
  • thermoplastic resin member ( ⁇ ) (Izod impact strength with notch):
  • the impact strength (Izod impact strength with notch) of the thermoplastic grease member ( ⁇ ) is measured in accordance with the provisions of AS TMD256. However, if the size of the test piece obtained from the molded product 1 is insufficient, cut the test piece from the site of the molded product 1 where the width, thickness, and length can be taken as much as possible, and perform measurement. . In addition, when the material of the thermoplastic resin member (II) is specified, a test piece of the size specified in ASTMD256 is separately molded using the material, and measurement is performed using it. I prefer that.
  • a plate-shaped part having a width of 10 mm, a length of 64 mm, and a thickness of 1 mm is cut out from the thermoplastic resin member ( ⁇ ) portion of the molded product 1 and the notch shape processing described in ASTM D256 is performed.
  • the glass transition temperature Tg of polyester resin is measured based on the method described in ISOl 1357-2. In Examples described later, measurement was performed using a Pyris 1 DSC (Differential Scanning Calorimeter, manufactured by Pakin Elmer 1 Instruments Inc.) as a differential scanning calorimeter. The temperature elevation rate was 10 ° CZ, and the midpoint of the portion where the DSC curve showed a step change was the glass transition temperature Tg. When multiple Tg were observed in a mixture, etc., the lowest glass transition temperature Tg was adopted as the glass transition temperature Tg of the composition.
  • the melting point Tm of polyester resin is measured using a differential scanning calorimeter (DSC). Later In this example, a sealed sample container with a capacity of 50 1 is filled with 1 mg to 5 mg of sample, heated from a temperature of 30 ° C to a temperature of 350 ° C at a heating rate of 10 ° CZ, and a melting point Tm was measured.
  • DSC differential scanning calorimeter
  • Pyris 1 DSC Perkin Elmer's Instruments differential scanning calorimeter
  • melt viscosity 1 of polyester resin has a dynamic viscoelasticity measuring device with a diameter of 2
  • Polyester resin at a specified temperature (temperature (Tm + 10) ° C) using a parallel plate of Omm, with a distance of 1. Omm, a measurement frequency of 0.5 Hz, and a generated torque of 0.005 J. Measure the viscoelasticity of the components and read the melt viscosity r? In Examples described later, 3 g of a polyester resin component was used, and measurement was performed using a dynamic viscoelasticity measuring apparatus ARES manufactured by T'A Instruments Inc. as a dynamic viscoelasticity measuring apparatus.
  • the melt viscosity 2 of polyester resin is measured using a dynamic viscoelasticity measuring device, using a parallel plate with a diameter of 2 Omm, distance between parallel plates 1. Omm, measurement frequency 0.5Hz, generated torque 0.005J Under the conditions described above, the viscoelasticity of the polyester resin component is measured at a predetermined temperature (250 ° C), and the melt viscosity r-2 is read. In Examples described later, 3 g of the polyester rosin component was used, and measurement was performed using a dynamic viscoelasticity measuring device ARES manufactured by TEA Instruments Co., Ltd. as a dynamic viscoelasticity measuring device.
  • the number average molecular weight of polyester resin is determined by gel permeation chromatography (GP
  • the number average molecular weight is different, that is, when there are two distributions of the number average molecular weight, from the viewpoint of evaluating the strength of the polyester resin. Of these, the lowest number average molecular weight is treated as the number average molecular weight of the polyester resin.
  • GPC-244 manufactured by WATERS was used as gel permeation chromatography (GPC).
  • Tear strength of impact resistant layer As a rule, tear strength is measured in accordance with IS06383-1. However, if the impact-resistant layer specimen obtained from the fiber-reinforced composite material (I) is not large enough, the fiber-reinforced composite material (I) can have a large width, thickness, and length as much as possible. Cut out a test piece from the impact-resistant layer and measure it. In addition, when the material of the impact resistant layer can be specified, it is preferable to separately measure the size of the test piece defined in IS06383-1 using the material and measure it.
  • a square test piece with a side length of 30 mm to 100 mm cut out from the fiber reinforced composite material (I) restrain the four sides within the range of 5 mm to 20 mm with the widest possible clamp width. Support the specimen so that it does not move.
  • a 5 kg steel striker with a hemispherical tip with a diameter of 16 mm is dropped from a height of 75 cm, and after a shock is applied, a through hole opens in the test piece.
  • a penetration test was performed by fixing a test piece having a size of 30 mm ⁇ 30 mm with a constraint width of 5 mm on all four sides.
  • Radio wave permeability is measured based on the Advantest method.
  • a square flat plate is cut out from the mobile phone housing to make a test piece.
  • the size of the test piece is preferably as large as possible.
  • the size of the test piece is preferably at least 20 mm ⁇ 20 mm. If the size of the test piece cannot be secured, the relevant material portion can be cut out and re-formed by hot press molding etc. so that the thickness is the same as that of the frame member. If the material is denatured by heat or cannot be reshaped, the composition of the corresponding material can be analyzed, and a material of the same composition can be formed into a test piece shape for measurement.
  • the fiber reinforced composite material (I) is cut out from the molded body 1 (cell phone casing 61). At that time, ribs, hinges, and parts provided with uneven shapes are avoided as much as possible. When these parts are included, these parts are cut off and used for the test.
  • the test piece should be cut out from at least two different angles. Preferably 3 directions, more preferably 4 directions.
  • the angle of each specimen is preferably 90 ° different for 2-way cutout, 60 ° different for 3-way cutout, and 45 ° different for 4-way cutout.
  • the size of the test piece preferably conforms to the provisions of IS0178. If it is not possible to secure a specimen of the specified size! / Or if the required number of specimens cannot be secured, cut out a large specimen as much as possible and make it available for measurement. It is preferable that a specimen with a width of at least 5mm and a length of 20mm can be secured. If a specimen that conforms to the standard cannot be secured, cut out a specimen that has a reduced ratio of width to length with respect to the standard, and keep the actual thickness. In this case, the span (distance between fulcrums) at the time of measurement is determined by reducing in proportion to the length of the test piece. Prepare 3 to 5 specimens for measurement. Other measurement conditions conform to the provisions of ISO 178.
  • the 0 ° and 90 ° directions are taken as the length direction of the test piece from the portion of the fiber reinforced composite material (I) of the cellular phone case 61 shown in FIGS. 6 and 7.
  • a test piece having a width of 8 mm and a length of 30 mm was cut out.
  • the number of test specimens was 3 in each direction.
  • “Instron” (registered trademark) 5565 type universal material testing machine (manufactured by Instron Japan) was used as a measuring device.
  • the tensile test was conducted at an ambient temperature of 25 ° C in a test room where the ambient temperature was adjustable.
  • the specimen Prior to the start of the test, the specimen was kept in a state where the tensile test load was not applied for at least 5 minutes in the test room, and a thermocouple was placed on the specimen to make it equivalent to the ambient temperature. After confirming the above, a bending test was conducted. The bending test was performed at an indenter speed of 1.27 mmZ. The bending elastic modulus of the test piece was calculated from the result of the bending test.
  • DICY7 (dicyandiamide, manufactured by Japan Epoxy Resin Co., Ltd.).
  • Bee-Leck (registered trademark)” K polybule formal, manufactured by Chisso Corporation.
  • T700SC-12K-50C tensile strength 4,900MPa, tensile modulus 235GPa, fiber specific gravity 1.80
  • epoxy resin composition Preparation method of uncured resin composition of matrix resin containing epoxy resin (in this example, abbreviated as epoxy resin composition):
  • the raw materials shown below were mixed with a kneader according to the composition ratio and procedure shown below to obtain an epoxy resin composition in which polyvinyl formal was uniformly dissolved.
  • the epoxy resin composition was coated on release paper using a reverse roll coater to prepare a resin film.
  • the coating amount of the epoxy resin composition per unit area of the resin film was 31 g / m 2 .
  • the carbon fiber “Torre force (registered trademark)” T700SC-12K-50C (made by Toray Industries, Inc.) aligned in one direction in a sheet shape so that the fiber weight per unit area becomes 125 gZm 2
  • a unidirectional prepreg was prepared by impregnating the epoxy resin composition in a gap between carbon fibers by applying the above-mentioned resin film on both sides to a tensile strength of 4,900 MPa and a tensile modulus of 230 GPa, and applying heat and pressure.
  • Copolyester resin (“Hytrel” (registered trademark) 2551, made by Toray DuPont Co., Ltd., melting point 164 ° C) and copolyester resin ("Kemid '(registered trademark) R248, manufactured by Toray Industries, Inc.), melting point 113 )
  • a JSW TEX-30a type twin screw extruder screw diameter 30mm, die diameter 5mm, barrel temperature 200 ° C, rotation speed 150rpm. It was extruded continuously, cooled, and then cut into 5 mm lengths with a cutter to obtain a polyester resin, which was press-developed at a temperature of 200 ° C and a pressure of 50 MPa, with a thickness of 60 A ⁇ m film was obtained.
  • the unidirectional carbon fiber pre-preparer prepared above has a predetermined size (300mm x 300mm) Cut to size, the direction along one side is 0 ° direction, fiber direction is from bottom to top, 0 °, 90 °, 0 ° Fifteen pre-predas were laminated so as to be 90 ° and 0 °.
  • This laminate is used for forming the fiber-reinforced composite material (I).
  • the prepreg laminate is set in a press die, and is cured by heating at a temperature of 160 ° C for 30 minutes while applying IMPa pressure.
  • a fiber reinforced composite material (I) is used as a fiber reinforced composite material (I).
  • the laminate of the thermoplastic resin (A) and the fiber reinforced composite material (I) obtained in (2) above has a predetermined size (the fiber direction of the outermost layer of the fiber reinforced composite material (I) is 0 °. (A rectangle with a direction of 280 mm and a fiber direction of the outermost layer of 90 ° and a direction of 210 mm) was set in an insert mold for injection molding. At this time, the thermoplastic resin (A) was arranged so as to come to the bonding surface.
  • thermoplastic resin component (coffin) was injection-molded as a thermoplastic resin component (coffin) to produce a fiber-reinforced composite material.
  • a molded product 41 for a personal computer casing as shown in FIG. 4 was manufactured by integrating with (I). In FIG. 4, the illustration of the thermoplastic resin (A) is omitted.
  • Copolymerized polyester resin (“Chemid” (registered trademark) Q1500, melting point 170 ° C., manufactured by Toray Industries, Inc.) was press-molded at a temperature of 200 ° C. and a pressure of 50 MPa to obtain a film having a thickness of 60 ⁇ m.
  • Example 2 The same as Example 1 except that the film of the thermoplastic resin (A) prepared in (1) above was used. Thus, a fiber reinforced composite material (I) and a laminate of the thermoplastic resin (A) and the fiber reinforced composite material (I) were obtained.
  • a personal computer case as shown in FIG. 4 is used in the same manner as in Example 1 except that the laminate of the fiber reinforced composite material (I) obtained in (2) above and the thermoplastic resin (A) is used. Manufactured product for body 41 was manufactured. From the part of the molded article 41 where the fiber reinforced composite material (I) and the thermoplastic resin member (II) were integrated, a test piece for measuring impact adhesive strength and adhesive strength was cut out. The measurement results are shown in Table 2.
  • thermoplastic resin (A) was prepared.
  • a molded product 41 for a personal computer casing as shown in FIG. 4 was obtained. From the part of the molded article 41 where the fiber reinforced composite material (I) and the thermoplastic resin member (II) were integrated, test pieces for evaluation of impact adhesive strength and adhesive strength were cut out. The measurement results are shown in Table 3.
  • thermoplastic resin (A) was prepared.
  • the unidirectional carbon fiber pre-preparer prepared above has a predetermined size (300mm x 300mm) Cut to size, the direction along one side is 0 ° direction, fiber direction is from bottom to top, 0 °, 90 °, 0 ° Fifteen pre-predas were laminated so as to be 90 ° and 0 °.
  • This laminate is used for forming the fiber-reinforced composite material (I). From the laminated prepredder, one sheet of the thermoplastic resin (A) film prepared in the above (1) cut to the same size as the prepreg laminated body was laminated and laminated.
  • thermoplastic resin (A) film prepared in (1) above cut to the same size as the pre-preda laminate is laminated and laminated.
  • a polyester resin film (“Lumirror” (registered trademark) HT50, tear strength 270 NZmm, thickness 100 m) manufactured by Toray Industries, Inc. is made to have the same size as the pre-preda laminate as an impact resistant layer. The cut pieces were stacked one on top of the other.
  • the prepreg laminate is set in a press die, and is cured by heating at a temperature of 160 ° C for 30 minutes while applying IMPa pressure.
  • a fiber reinforced composite material (I) is used as a fiber reinforced composite material (I).
  • a personal computer case as shown in FIG. 4 is used in the same manner as in Example 1 except that the laminate of the fiber reinforced composite material (I) obtained in (2) above and the thermoplastic resin (A) is used.
  • Manufactured product for body 41 was manufactured. From the part of the molded article 41 where the fiber reinforced composite material (I) and the thermoplastic resin member (II) were integrated, a test piece for measuring impact adhesive strength and adhesive strength was cut out. Further, a test piece for measurement of penetration test was cut out from the fiber reinforced composite material (I). The measurement results are shown in Table 4.
  • thermoplastic resin (A) was prepared.
  • Example 1 except that GFZ polycarbonate resin (manufactured by Nippon GEP Co., Ltd., Lexan 3412R. GF 20% by weight, Izod impact strength lOOjZm with notch) pellets was used as the thermoplastic resin component (II).
  • GFZ polycarbonate resin manufactured by Nippon GEP Co., Ltd., Lexan 3412R. GF 20% by weight, Izod impact strength lOOjZm with notch
  • FIG. 4 A test piece for evaluation of impact adhesive strength and adhesive strength was cut out from the part of the molded product where the fiber reinforced composite material (I) and the thermoplastic resin member (resin) were integrated. The measurement results are shown in Table 5.
  • thermoplastic resin (A) was prepared.
  • the unidirectional carbon fiber pre-preparer prepared above is cut into a predetermined size (300mm x 300mm), the direction along one side is the 0 ° direction, and the fiber direction is from bottom to top. °, 90 °, 0 °. Fifteen pre-predas were laminated so as to be 90 ° and 0 °.
  • This laminate is used for forming the fiber-reinforced composite material (I).
  • the prepreg laminate is set in a press mold, heated and cured at a temperature of 160 ° C for 30 minutes while applying IMPa pressure, and then the thermoplastic material prepared in (1) above is applied to the cured plate.
  • the resin (A) was laminated and press-molded at a temperature of 160 ° C. for 1 minute to obtain a fiber-reinforced composite material (I).
  • a personal computer case as shown in FIG. 4 is used in the same manner as in Example 1 except that the laminate of the fiber reinforced composite material (I) obtained in (2) above and the thermoplastic resin (A) is used. Manufactured products for body use. A test specimen for measuring the impact adhesive strength and the adhesive strength was cut out from the part of the molded article in which the fiber reinforced composite material (I) and the thermoplastic resin member (resin) were integrated. The measurement results are shown in Table 6.
  • thermoplastic resin (A) film prepared in (1) above the fiber reinforced composite material (1), and the thermoplastic resin (A) and fiber reinforced resin were used in the same manner as in Example 1.
  • Composite material (A) is the thermoplastic resin (A) film prepared in (1) above, the fiber reinforced composite material (1), and the thermoplastic resin (A) and fiber reinforced resin were used in the same manner as in Example 1.
  • a personal computer case as shown in FIG. 4 is used in the same manner as in Example 1 except that the laminate of the fiber reinforced composite material (I) obtained in (2) above and the thermoplastic resin (A) is used. Manufactured product for body 41 was manufactured. The fiber reinforced composite material (I) and thermoplastic resin component (II) of this molded product 41
  • Copolymerized polyester resin (“Chemisdo” (registered trademark) K1089 manufactured by Toray Industries, Inc., melting point 135 ° C) and copolymerized polyester resin (“Chemisdo” (registered trademark) R248 manufactured by Toray Industries, Inc.), melting point 113 ° C ) And GEX using a JSW TEX-30a type twin screw extruder (screw diameter 30mm, die diameter 5mm, barrel temperature 200 ° C, rotation speed 150rpm). This was extruded continuously, cooled, and then cut into 5 mm lengths with a cutter to obtain polyester resin. This polyester resin was press-molded at a temperature of 200 ° C. and a pressure of 50 MPa to obtain a film having a thickness of 60 ⁇ m.
  • thermoplastic resin (A) film prepared in (1) above the fiber reinforced composite material (1), and the thermoplastic resin (A) and fiber reinforced resin were used in the same manner as in Example 1. A laminate with composite material (I) was obtained.
  • a personal computer case as shown in FIG. 4 is used in the same manner as in Example 1 except that the laminate of the fiber reinforced composite material (I) obtained in (2) above and the thermoplastic resin (A) is used.
  • Body use Form 41 was manufactured. From the part of the molded article 41 where the fiber reinforced composite material (I) and the thermoplastic resin member (II) were integrated, a test piece for measuring impact adhesive strength and adhesive strength was cut out. The measurement results are shown in Table 8.
  • Example 4 As described above, in Examples 1 to 4, it was possible to produce molded articles having excellent impact resistance, but in Comparative Example 1, the impact resistance of the thermoplastic resin member ( ⁇ ) was low. When measuring the impact bond strength of bad joints, the thermoplastic resin member (good) caused the base material to break, and the molded article had poor impact resistance. Furthermore, in Example 4, since the fiber-reinforced composite material (I) had an impact resistant layer, the produced molded article had excellent penetration resistance. [0164] On the other hand, in Comparative Example 2, since there is no maximum impregnation thickness h of the thermoplastic resin (A), it is easy between the fiber-reinforced composite material (I) and the thermoplastic resin member (resin). The molded product was extremely poor in impact resistance.
  • Comparative Example 3 since the tensile strength at break of the thermoplastic resin (A) was low, the molded article had poor impact resistance. Further, in Comparative Example 4, since the tensile elongation at break of the thermoplastic resin (A) was low, the molded article had poor impact resistance. The molded products manufactured in Comparative Examples 1 to 4 were difficult to apply to electrical / electronic equipment casings that require extremely high impact resistance.
  • Copolyester resin (“Hytrel” (registered trademark) 2551, made by Toray DuPont Co., Ltd., melting point 164 ° C) and copolyester resin ("Kemid '(registered trademark) R248, manufactured by Toray Industries, Inc.), melting point 113 )
  • a JSW TEX-30a type-shaft extruder screw diameter 30mm, die diameter 5mm, barrel temperature 200 ° C, rotation speed 150rpm. After being continuously extruded and cooled, it was cut to a length of 5 mm with a cutter to obtain a polyester resin, which was press-molded at a temperature of 200 ° C and a pressure of 50 MPa to obtain a film. .
  • the unidirectional carbon fiber pre-preparer prepared above is cut into a predetermined size (300mm x 300mm), the direction along one side is the 0 ° direction, and the fiber direction is from top to bottom.
  • Three pre-predas were laminated so as to be 90 ° and 0 °.
  • one piece of the thermoplastic resin (A) film prepared in the above (1) cut to the same size as the prepreg laminate was laminated and laminated.
  • the pre-preder laminate is set in a press die, heated and cured at a temperature of 160 ° C for 30 minutes while applying pressure of IMPa, press-molded, and a fiber-reinforced composite material (I )
  • thermoplastic resin (A) thermoplastic resin (thermal bonding substrate) was located on the bonding surface.
  • Polycarbonate resin manufactured by Nippon GEP Co., Ltd., Lexan 141R pellets is injection-molded as a thermoplastic resin (frame part) (frame) and integrated with the fiber reinforced composite material (I).
  • Table 9 shows the measurement results of various characteristic values of the cellular phone housing 61.
  • a film was obtained in the same manner as in Example 2, (1).
  • a mobile phone case 61 as shown in FIGS. 6 and 7 was manufactured.
  • Table 10 shows the measurement results of various characteristic values of the cellular phone casing 61.
  • the fiber was cut using a thermoplastic resin (A) and the unidirectional carbon fiber pre-preda was cut into a size of a predetermined size (300mm x 300mm), and the direction along one side was the 0 ° direction.
  • Directional force S Other than laminating 9 pre-predas so that the upward force is lower than the upward force ⁇ , 0 °, 90 °, 0, 90 °, 0 ° 90 °, 0 °, 90 °, 0 °
  • a fiber-reinforced composite material (I) was obtained.
  • Thermoplastic ⁇ member (frame portion) (II), GFZ polycarbonate ⁇ (Nippon G EP (Ltd.), Lexan 3412R, GF20 weight 0/0) Leave injection molding in advance a frame shape pellets, the The fiber reinforced composite material (I) obtained in (1) and the frame part ( ⁇ ) are joined using a one-pack type epoxy adhesive (EW2070, manufactured by Sumitomo 3EM Co., Ltd.).
  • EW2070 manufactured by Sumitomo 3EM Co., Ltd.
  • a fiber reinforced composite material (I) was obtained in the same manner as (2) of Example 2 except that the thermoplastic resin (A) was not used.
  • Thermoplastic ⁇ member (frame portion) (II), GFZ polycarbonate ⁇ (Nippon G EP (Ltd.), Lexan 3412R. GF20 weight 0/0) was injection molding in advance a frame shape pellets. At this time, molding was performed using a mold having a joint area with the fiber-reinforced composite material (I) of 120 mm 2 .
  • the fiber reinforced composite material (I) obtained in (1) above and the frame part (II) are joined using a one-pack type epoxy adhesive (manufactured by Sumitomo 3EM Co., Ltd., EW2070).
  • a mobile phone casing as shown in FIG. Table 12 shows the measurement results of various characteristics of this mobile phone casing.
  • the molded article of the present invention is preferably used in electrical and electronic equipment, office automation equipment, home appliances, medical equipment, automobile parts, aircraft parts or building materials that require impact resistance.

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Abstract

L'invention concerne un article moulé comprenant une matière composite renforcée par des fibres (I) contenant une fibre de renforcement continu et une résine matricielle thermodurcissable ainsi qu'un élément (II) en résine thermoplastique relié et intégré à au moins une partie de la surface de la matière (I) composite renforcée par des fibres à l'aide d'une résine thermoplastique (A). La surface reliée entre la résine thermoplastique (A) et la matière (I) composite renforcée par des fibres comporte des projections et des cavités en coupe transversale dans la direction de l'épaisseur de l'article moulé ; la profondeur d'imprégnation maximale h de la résine thermoplastique (A) dans la matière (I) composite renforcée par des fibres n'est pas inférieure à 10 µm. La résine thermoplastique (A) présente une résistance à la rupture par traction supérieure ou égale à 25 MPa et un allongement à la rupture par traction supérieure ou égale à 200 %. La résistance aux adhésifs de contact au niveau de la partie reliée de la matière (I) composite renforcée par des fibres et de l'élément en résine thermoplastique (II) est supérieure ou égale à 3 000 J/m².
PCT/JP2007/064240 2006-07-28 2007-07-19 Article moulé et son procédé de fabrication Ceased WO2008013094A1 (fr)

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EP2100719A1 (fr) * 2008-03-12 2009-09-16 BYD Company Limited Matériau composite en fibres de carbone, produit et procédé
WO2021199906A1 (fr) * 2020-03-31 2021-10-07 東レ株式会社 Résine renforcée par des fibres, article moulé intégré et procédé de production de résine renforcée par des fibres
CN114103340A (zh) * 2021-12-23 2022-03-01 浙江远景体育用品有限公司 一种连续纤维增强热塑性头盔外壳材料及制备方法

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